A modular table-top setup for ultrafast x-ray diffraction.

We present a table-top setup for femtosecond time-resolved x-ray diffraction based on a Cu Kα (8.05 keV) laser driven plasma x-ray source. Due to its modular design, it provides high accessibility to its individual components (e.g., x-ray optics and sample environment). The Kα-yield of the source is optimized using a pre-pulse scheme. A magnifying multilayer x-ray mirror with Montel-Helios geometry is used to collect the emitted radiation, resulting in a quasi-collimated flux of more than 105 Cu Kα photons/pulse impinging on the sample under investigation at a repetition rate of 10 Hz. A gas ionization chamber detector is placed right after the x-ray mirror and used for the normalization of the diffraction signals, enabling the measurement of relative signal changes of less than 1% even at the given low repetition rate. Time-resolved diffraction experiments on laser-excited epitaxial Bi films serve as an example to demonstrate the capabilities of the setup. The setup can also be used for Debye-Scherrer type measurements on poly-crystalline samples.

Implementation and operation of a fiber-coupled CMOS detector in a low energy electron Microscope.

The intrinsically weak signals in ultrafast electron microscopy experiments demand an improvement in the signal-to noise ratio of suitable electron detectors. We provide an experience report describing the installation and operation of a fiber-coupled CMOS based detector in a low energy electron microscope. We compare the detector performance to the traditional multi-channel-plate-based setup. The high dynamic range CMOS detector is capable of imaging spatially localized large intensity variations with low noise. The detector is blooming-free and overexposure appears uncritical. Overall, we find dramatic improvements in the imaging with the fiber-coupled CMOS detector compared to imaging with our previously used multi-channel-plate detector.

High Layer Uniformity of Two-Dimensional Materials Demonstrated Surprisingly from Broad Features in Surface Electron Diffraction.

Paradoxically, a very broad diffraction background, named the bell-shaped-component (BSC), has been established as a feature of graphene growth. Recent diffraction studies as a function of electron energy have shown that the BSC is not related to scattering interference. Here, additional experiments are carried out as a function of temperature over the range in which single-layer graphene (SLG) grows. Quantitative fitting of the profiles shows that the BSC follows the increase of the Gr(10) spot, proving directly that the BSC indicates high-quality graphene. Additional metal deposition experiments provide more information about the BSC. The BSC is insensitive to metal deposition, and it increases with metal intercalation, because a more uniform interface forms between graphene and SiC. These experiments support the conclusion that the BSC originates from electron confinement within SLG, and surprisingly, it is an excellent measure of graphene uniformity.

Thermally Induced Crossover from 2D to 1D Behavior in an Array of Atomic Wires: Silicon Dangling-Bond Solitons in Si(553)-Au.

The self-assembly of submonolayer amounts of Au on the densely stepped Si(553) surface creates an array of closely spaced "atomic wires" separated by 1.5 nm. At low temperature, charge transfer between the terraces and the row of silicon dangling bonds at the step edges leads to a charge-ordered state within the row of dangling bonds with ×3 periodicity. Interactions between the dangling bonds lead to their ordering into a fully two-dimensional (2D) array with centered registry between adjacent steps. We show that as the temperature is raised, soliton defects are created within each step edge. The concentration of solitons rises with increasing temperature and eventually destroys the 2D order by decoupling the step edges, reducing the effective dimensionality of the system to 1D. This crossover from higher to lower dimensionality is unexpected and, indeed, opposite to the behavior in other systems.

Decelerated lattice excitation and absence of bulk phonon modes at surfaces: Ultra-fast electron diffraction from Bi(111) surface upon fs-laser excitation.

Ultrafast reflection high-energy electron diffraction is employed to follow the lattice excitation of a Bi(111) surface upon irradiation with a femtosecond laser pulse. The thermal motion of the atoms is analyzed through the Debye-Waller effect. While the Bi bulk is heated on time scales of 2 to 4 ps, we observe that the excitation of vibrational motion of the surface atoms occurs much slower with a time constant of 12 ps. This transient nonequilibrium situation is attributed to the weak coupling between bulk and surface phonon modes which hampers the energy flow between the two subsystems. From the absence of a fast component in the transient diffraction intensity, it is in addition concluded that truncated bulk phonon modes are absent at the surface.

Condensation of ground state from a supercooled phase in the Si(111)-(4 × 1) → (8 × 2)-indium atomic wire system.

Strong optical irradiation of indium atomic wires on a Si(111) surface causes the nonthermal structural transition from the (8 × 2) reconstructed ground state to an excited (4 × 1) state. The immediate recovery of the system to the ground state is hindered by an energy barrier for the collective motion of the indium atoms along the reaction coordinate from the (4 × 1) to the (8 × 2) state. This metastable, supercooled state can only recover through nucleation of the ground state at defects like adsorbates or step edges. Subsequently, a recovery front propagates with constant velocity across the surface and the (8 × 2) ground state is reinstated. In a combined femtosecond electron diffraction and photoelectron emission microscopy study, we determined-based on the step morphology-a velocity of this recovery front of ∼100 m/s.

Ultrafast electron diffraction from a Bi(111) surface: Impulsive lattice excitation and Debye-Waller analysis at large momentum transfer.

The lattice response of a Bi(111) surface upon impulsive femtosecond laser excitation is studied with time-resolved reflection high-energy electron diffraction. We employ a Debye-Waller analysis at large momentum transfer of 9.3 Å-1 ≤ Δ k ≤ 21.8 Å-1 in order to study the lattice excitation dynamics of the Bi surface under conditions of weak optical excitation up to 2 mJ/cm2 incident pump fluence. The observed time constants τ int of decay of diffraction spot intensity depend on the momentum transfer Δk and range from 5 to 12 ps. This large variation of τ int is caused by the nonlinearity of the exponential function in the Debye-Waller factor and has to be taken into account for an intensity drop ΔI > 0.2. An analysis of more than 20 diffraction spots with a large variation in Δk gave a consistent value for the time constant τT of vibrational excitation of the surface lattice of 12 ± 1 ps independent on the excitation density. We found no evidence for a deviation from an isotropic Debye-Waller effect and conclude that the primary laser excitation leads to thermal lattice excitation, i.e., heating of the Bi surface.

Pulsed electron gun for electron diffraction at surfaces with femtosecond temporal resolution and high coherence length.

We present a newly designed 30 kV pulsed electron gun for ultrafast electron diffraction suited for pump-probe setups driven by femtosecond laser pulses. The electron gun can be operated both in transmission and reflection geometry. A robust design with a back illuminated Au photocathode, extraction fields of 7.5 kV/mm, and a magnetic focus lens ensures reliable daily use. Magnetic deflectors allow for beam alignment and characterization. Focusing of the UV pulse on the photocathode results in a small source size of photoemitted electrons and thus a high transverse coherence length of more than 50 nm in diffraction. A low difference of ΔE = 0.1 eV between the work function of the 10 nm Au photocathode and photon energy of the frequency tripled UV laser pulses results in an instrumental temporal resolution of 330 fs full width at half maximum. This resolution is discussed with respect to the number of electrons per pulse.

Non-equilibrium lattice dynamics of one-dimensional In chains on Si(111) upon ultrafast optical excitation.

The photoinduced structural dynamics of the atomic wire system on the Si(111)-In surface has been studied by ultrafast electron diffraction in reflection geometry. Upon intense fs-laser excitation, this system can be driven in around 1 ps from the insulating [Formula: see text] reconstructed low temperature phase to a metastable metallic [Formula: see text] reconstructed high temperature phase. Subsequent to the structural transition, the surface heats up on a 6 times slower timescale as determined from a transient Debye-Waller analysis of the diffraction spots. From a comparison with the structural response of the high temperature [Formula: see text] phase, we conclude that electron-phonon coupling is responsible for the slow energy transfer from the excited electron system to the lattice. The significant difference in timescales is evidence that the photoinduced structural transition is non-thermally driven.

Optically excited structural transition in atomic wires on surfaces at the quantum limit.

Transient control over the atomic potential-energy landscapes of solids could lead to new states of matter and to quantum control of nuclear motion on the timescale of lattice vibrations. Recently developed ultrafast time-resolved diffraction techniques combine ultrafast temporal manipulation with atomic-scale spatial resolution and femtosecond temporal resolution. These advances have enabled investigations of photo-induced structural changes in bulk solids that often occur on timescales as short as a few hundred femtoseconds. In contrast, experiments at surfaces and on single atomic layers such as graphene report timescales of structural changes that are orders of magnitude longer. This raises the question of whether the structural response of low-dimensional materials to femtosecond laser excitation is, in general, limited. Here we show that a photo-induced transition from the low- to high-symmetry state of a charge density wave in atomic indium (In) wires supported by a silicon (Si) surface takes place within 350 femtoseconds. The optical excitation breaks and creates In-In bonds, leading to the non-thermal excitation of soft phonon modes, and drives the structural transition in the limit of critically damped nuclear motion through coupling of these soft phonon modes to a manifold of surface and interface phonons that arise from the symmetry breaking at the silicon surface. This finding demonstrates that carefully tuned electronic excitations can create non-equilibrium potential energy surfaces that drive structural dynamics at interfaces in the quantum limit (that is, in a regime in which the nuclear motion is directed and deterministic). This technique could potentially be used to tune the dynamic response of a solid to optical excitation, and has widespread potential application, for example in ultrafast detectors.

Spot profile analysis and lifetime mapping in ultrafast electron diffraction: Lattice excitation of self-organized Ge nanostructures on Si(001).

Ultrafast high energy electron diffraction in reflection geometry is employed to study the structural dynamics of self-organized Germanium hut-, dome-, and relaxed clusters on Si(001) upon femtosecond laser excitation. Utilizing the difference in size and strain state the response of hut- and dome clusters can be distinguished by a transient spot profile analysis. Surface diffraction from {105}-type facets provide exclusive information on hut clusters. A pixel-by-pixel analysis of the dynamics of the entire diffraction pattern gives time constants of 40, 160, and 390 ps, which are assigned to the cooling time constants for hut-, dome-, and relaxed clusters.

Ultra-fast electron diffraction at surfaces: from nanoscale heat transport to driven phase transitions.

Many fundamental processes of structural changes at surfaces occur on a pico- or femtosecond time scale. In order to study such ultra-fast processes, we have combined modern surface science techniques with fs-laser pulses in a pump-probe scheme. Reflection high energy electron diffraction (RHEED) with grazing incident electrons ensures surface sensitivity for the probing electron pulses. Utilizing the Debye-Waller effect, we studied the cooling of vibrational excitations in monolayer adsorbate systems or the nanoscale heat transport from an ultra-thin film through a hetero-interface on the lower ps-time scale. The relaxation dynamics of a driven phase transition far away from thermal equilibrium is demonstrated with the In-induced (8×2) reconstruction on Si(111). This surface exhibits a Peierls-like phase transition at 100K from a (8×2) ground state to (4×1) excited state. Upon excitation by a fs-laser pulse, this structural phase transition is driven into an excited (4×1) state at a sample temperature of 20K. Relaxation into the (8×2) ground state occurs after more than 150 ps.

Manipulation of electronic transport in the Bi(111) surface state.

We demonstrate the controlled manipulation of the 2D-electronic transport in the surface state of Bi(111) through the deposition of small amounts of Bi to generate adatoms and 2D islands as additional scatterers. The corresponding increase in resistance is recorded in situ and in real time. Model calculations based on mean-field nucleation theory reveal a constant scattering efficiency of adatoms and of small 2D Bi islands, independent of their size. This finding is supported by a detailed scanning tunneling microscopy and spectroscopy study at 5 K which shows a highly anisotropic scattering pattern surrounding each surface protrusion.

Lost in reciprocal space? Determination of the scattering condition in spot profile analysis low-energy electron diffraction.

The precise knowledge of the diffraction condition, i.e., the angle of incidence and electron energy, is crucial for the study of surface morphology through spot profile analysis low-energy electron diffraction (LEED). We demonstrate four different procedures to determine the diffraction condition: employing the distortion of the LEED pattern under large angles of incidence, the layer-by-layer growth oscillations during homoepitaxial growth, a G(S) analysis of a rough surface, and the intersection of facet rods with 3D Bragg conditions.

Epitaxial Ag wires with a single grain boundary for electromigration.

Test structures for electromigration with defined grain boundary configurations can be fabricated using focused ion beam (FIB). We present a novel approach of combining epitaxial growth of Ag islands with FIB milling. Depending on the growth parameters, bi-crystalline Ag islands can be grown on Si(111) surfaces and can be structured into wires by FIB. To avoid doping effects of the used Ga FIB, silicon on insulator (SOI) substrates are used. By cutting through the device layer of the SOI substrate with deep trenches, the Ag wire can be electrically separated from the rest of the substrate. In this way, Ag wires with one isolated grain boundary of arbitrary direction can be assembled. Using scanning electron microscopy we demonstrate the feasibility of our approach.

Space charge effects in photoemission electron microscopy using amplified femtosecond laser pulses.

Linear and nonlinear photoemission microscopy is used to study the origin of space charge effects that are frequently observed if amplified femtosecond lasers are used for generation of photoelectrons. Space charge effects are apparent in the width of the photoemission spectra, but also create image blur. The onset threshold for space charge effects is determined by recording the width of photoemission spectra and by finding the conditions under which spectral broadening is just less than the energy resolution of the microscope. The principal findings are independent if harmonics of the fundamental of the fs laser pulses are used, but the space charge effects are found to be more dominant at lower repetition rates. By inserting apertures into the electron path, the place at which space charge effects occur can be localized.

The influence of anisotropic diffusion on Ag nanowire formation.

Photoemission electron microscopy is used to study the growth of single-crystalline silver nanowires on flat and vicinal Si(001) substrates. The growth experiments were performed at various temperatures and showed a temperature dependence of nanowire formation. The nanowires on Si(001) are evenly distributed in the [110] and [Formula: see text] directions on the surface, whereas on a 4° vicinal surface the wires grow only along the steps, in the [Formula: see text] direction. This change in wire distribution is attributed to the increasing diffusion anisotropy as the vicinality of the substrate increases.

Real-time view of mesoscopic surface diffusion.

Photoemission electron microscopy is used to study the thermal decay of Ag islands grown epitaxially on Si(001) surfaces. (2 x 3) Ag reconstructed zones, due to migrating Ag atoms supplied to the surface by the decaying islands, surround each of the islands. The shape of these reconstructed zones depends on the degree of diffusion isotropy in the system. We demonstrate that the imaging of these reconstructed "isocoverage zones" constitutes a unique experimental method for directly observing diffusion fields in epitaxial systems. We describe the dynamics of the thermal decay of the islands and the isozones in the context of a continuum diffusion model.

A pulsed electron gun for ultrafast electron diffraction at surfaces.

The construction of a pulsed electron gun for ultrafast reflection high-energy electron diffraction experiments at surfaces is reported. Special emphasis is placed on the characterization of the electron source: a photocathode, consisting of a 10 nm thin Au film deposited onto a sapphire substrate. Electron pulses are generated by the illumination of the film with ultraviolet laser pulses of femtosecond duration. The photoelectrons are emitted homogeneously across the photocathode with an energy distribution of 0.1 eV width. After leaving the Au film, the electrons are accelerated to kinetic energies of up to 15 keV. Focusing is accomplished by an electrostatic lens. The temporal resolution of the experiment is determined by the probing time of the electrons traveling across the surface which is about 30 ps. However, the duration of the electron pulses can be reduced to less than 6 ps.